Gas supply device and gas supply method

Abstract

To provide an efficient gas supply device and gas supply method. [Solution] The supply device 100 comprises a gas separation membrane 1 that permeates the product gas, a gas separation container 2 that houses the separation membrane 1, and a heating device 20 that heats the separation membrane 1. The gas separation container 2 has a first space 31 for storing the raw material solution of the product gas, a second space 32 partitioned from the first space 31 by the separation membrane 1, a carrier gas inlet 42 that communicates with the second space 32 and introduces carrier gas into the second space 32, and an outlet 44 that communicates with the second space 32 and sends out a mixed gas of carrier gas and product gas from the second space 32.

Description

Technical Field

[0001] The present invention relates to a gas supply device and a gas supply method.

Background Art

[0002] Due to the high integration of semiconductors, it is necessary to lower the temperature and improve the throughput of semiconductor manufacturing processes. For improving this throughput, highly reactive gases such as hydrogen peroxide and hydrazine are required as gases for semiconductor materials. However, these highly reactive gases are liable to decompose during transportation and storage. Therefore, these highly reactive gases may be transported and stored in the form of solutions in which these gases are dissolved in water or organic solvents in order to suppress decomposition during transportation and storage. For example, hydrogen peroxide may be transported and stored in the form of an aqueous solution, and hydrazine may be transported and stored in the form of a mixture (solution) with an organic solvent.

[0003] When a highly reactive gas is in the form of a solution as described above, it is necessary to separate these gases from this solution when using the highly reactive gas. However, when separating and using a highly reactive gas from such a solution, problems have arisen such that the concentration of these gases becomes low or the vapor of the solvent is mixed into these gases. Therefore, for example, as disclosed in Patent Document 1, a concentrated gas with an increased concentration may be obtained using a separation membrane, and this concentrated gas may be supplied to a device that uses the gas.

[0004] Patent Document 1 discloses a supply method and supply apparatus for supplying gaseous materials (product gas) used, for example, in the manufacture of semiconductor devices. This supply method includes a mixed gas preparation step of introducing a carrier gas into a container containing the material in solid or liquid form to obtain a mixed gas of the vaporized material and the carrier gas; a concentration step of obtaining a concentrated gas by increasing the concentration of the material in the mixed gas using a separation membrane; and a supply step of supplying the concentrated gas to an apparatus that uses the material. In this supply method, the carrier gas in the mixed gas permeates through the separation membrane, increasing the concentration of the material in the supplied mixed gas and resulting in a concentrated gas. Patent Document 1 discloses that, for example, gaseous materials used in the manufacture of semiconductor devices require high concentration. [Prior art documents] [Patent Documents]

[0005] [Patent Document 1] Japanese Patent Publication No. 2024-118353 [Overview of the project] [Problems that the invention aims to solve]

[0006] In the supply method and supply apparatus disclosed in Patent Document 1, as described above, a carrier gas is introduced into a container containing a gaseous material (hereinafter referred to as "product gas") used in a subsequent process, either in a solid or liquid state. A mixed gas is obtained from the vaporized product gas and the carrier gas, and then a separation membrane is used to increase the concentration of the product gas contained in this mixed gas. Therefore, for example, the amount of product gas that can be supplied is limited by the vaporization rate of the product gas from its solid or liquid state, and it may not be possible to efficiently supply a high-concentration product gas. In addition, because the product gas is further concentrated after obtaining the mixed gas, the process becomes complex, and therefore it may not be possible to efficiently supply a high-concentration product gas. Against this backdrop, there is a need for further efficiency improvements in gas supply apparatus and gas supply method for highly reactive gases.

[0007] This invention has been made in view of the above circumstances, and its purpose is to provide an efficient gas supply device and gas supply method. [Means for solving the problem]

[0008] The gas supply device according to the present invention for achieving the above objective is: A gas separation membrane that permeates the product gas, A gas separation container containing the separation membrane, The system includes a heating device for heating the separation membrane, The aforementioned gas separation container is A first space for storing the raw material solution of the product gas, The first space and the second space separated by the separation membrane, A carrier gas inlet that communicates with the second space and introduces carrier gas into the second space, It has an outlet that communicates with the second space and discharges a mixed gas of the carrier gas and the product gas from the second space.

[0009] The gas supply method according to the present invention for achieving the above objective is: A separation step involves bringing the raw material solution of the product gas into contact with a gas separation membrane and separating the product gas from the raw material solution by allowing it to pass through the separation membrane. A heating step for heating the separation membrane, The process includes a discharge step in which a carrier gas is introduced into the product gas separated in the separation step, and a mixed gas of the product gas and the carrier gas is discharged. The heating step is performed during the separation step. [Effects of the Invention]

[0010] According to this disclosure, it is possible to provide an efficient gas supply device and gas supply method. [Brief explanation of the drawing]

[0011] [Figure 1] This is an explanatory diagram of the configuration of the gas supply device (supply device) according to this embodiment. [Figure 2] This is an explanatory diagram illustrating the configuration of a gas supply device (supply device) according to another embodiment. [Modes for carrying out the invention]

[0012] Based on the drawings, a gas supply device and a gas supply method according to an embodiment of the present invention will be described.

[0013] First, an overview of the gas supply device and gas supply method according to this embodiment will be described.

[0014] Figure 1 shows an explanatory diagram of the configuration of a gas supply device 100, which is an example of a gas supply device according to this embodiment.

[0015] As shown in Figure 1, the supply device 100 includes a gas separation membrane 1 that permeates the product gas, a gas separation container 2 that houses the separation membrane 1, and a heating device 20 that heats the separation membrane 1. The gas separation container 2 has a first space 31 for storing the raw material solution of the product gas, a second space 32 separated from the first space 31 by the separation membrane 1, a carrier gas inlet 42 that communicates with the second space 32 and introduces carrier gas into the second space 32, and an outlet 44 that communicates with the second space 32 and delivers a mixed gas of carrier gas and product gas from the second space 32.

[0016] The gas supply method according to this embodiment includes a separation step of bringing a raw material solution of product gas into contact with a gas separation membrane 1 and separating the product gas from the raw material solution by allowing it to permeate the separation membrane 1; a heating step of heating the separation membrane 1; and a discharge step of introducing a carrier gas into the product gas separated in the separation step and discharging a mixed gas of the product gas and the carrier gas. The heating step is performed during the separation step.

[0017] The supply device 100 can efficiently supply gas containing product gas (mixed gas). More specifically, the supply device 100 can efficiently separate product gas from the raw material solution of the product gas, thereby enabling efficient supply of the mixed gas.

[0018] Also, according to the gas supply method according to the present embodiment, a gas (mixed gas) containing product gas can be efficiently supplied. The gas supply method according to the present embodiment can be realized by the supply device 100 as an example.

[0019] Hereinafter, the supply device 100 will be described in detail. Also, taking the case of using the supply device 100 as an example, the gas supply method according to the present embodiment will be described in detail.

[0020] The supply device 100 separates product gas from the raw material solution of the product gas supplied from an upstream device or the like at a high concentration (that is, in a state containing as little solvent component of the raw material solution as possible), and supplies a mixed gas of this product gas and a carrier gas to a device or the like on the downstream side of the process (for example, a semiconductor manufacturing device). In the present embodiment, the raw material solution is a solution containing a raw material component that is a raw material of the product gas. Also, the mixing of gas caused by the solvent of the raw material solution into the mixed gas is allowed. Also, the gas means being in a gaseous state. The concept of gas in the present embodiment includes the concept of vapor.

[0021] An example of the product gas is a highly reactive gas. For example, in the semiconductor manufacturing process, a highly reactive gas that is in great demand, that is, a highly reactive gas that is often used for semiconductor manufacturing in the semiconductor manufacturing process, is a gas having a highly polar molecular structure such as hydrazine, hydrogen peroxide, and formic acid (a gas of a polar molecule).

[0022] Preferred gases as the carrier gas are hydrogen, nitrogen, oxygen, helium, argon, and a gas obtained by mixing at least two or more of these gases.

[0023] The raw material solution is a solution containing a component (raw material component) of the product gas. That is, the raw material solution is a solution containing a raw material component composed of polar molecules as a raw material of the product gas.

[0024] Examples of raw material solutions are as follows: When the product gas is hydrazine, the raw material solution is a mixture of liquid hydrazine and an organic solvent (e.g., diglym (diethylene glycol dimethyl ether)). When the product gas is hydrogen peroxide, the raw material solution is hydrogen peroxide solution. When the product gas is formic acid, the raw material solution is an aqueous solution of formic acid.

[0025] The supply device 100 may, for example, include a separation membrane 1, a gas separation container 2, a heating device 20, a liquid level sensor 21, a liquid volume control mechanism 5, a concentration sensor 89, and a pressure control mechanism 6. In addition to the above, the supply device 100 may further include a raw material container 70, such as a storage tank (for example, a cushion tank) for temporarily storing the raw material solution to be supplied to the gas separation container 2.

[0026] The separation membrane 1 is a membrane-like component that allows the product gas in the raw material solution to permeate from one side of the membrane to the other side, while preventing the solvent in the raw material solution from permeating through, or making it extremely difficult for the solvent to permeate through. In other words, the separation membrane 1 is a membrane-like component that can separate (extract) the product gas from the raw material solution at a high concentration. Hereafter, the separation of the product gas from the raw material solution by permeating through the separation membrane 1 may be simply referred to as "separating the product gas from the raw material solution." By using the separation membrane 1, it is possible to separate the product gas from the raw material solution while suppressing the contamination of the solvent in the raw material solution.

[0027] The type of membrane used for separation membrane 1 may be appropriately selected depending on the product gas to be separated and the type of solvent in the raw material solution. It is preferable that separation membrane 1 does not allow gases other than the product gas to permeate, or allows them to permeate very little.

[0028] Suitable membrane members for separation membrane 1 include zeolite membranes and organometallic structure membranes (membranes formed from organometallic structure (MOF) materials). These membranes are particularly suitable for separating gases with highly polar molecular structures, such as hydrazine, hydrogen peroxide, and formic acid, because they have a high ability to selectively adsorb polar molecules. Separation membrane 1 may be a membrane member comprising at least one of the zeolite membrane and the organometallic structure membrane.

[0029] Among zeolite membranes, particularly preferred are CHA-type zeolite membranes, such as those using high-silica CHA-type zeolite based on porous aluminum oxide, for example, ZEBREX® ZX1 and ZX3 manufactured by Mitsubishi Chemical Corporation. The use of membranes using MFI-type zeolite is also not excluded. When a zeolite membrane is used as a separation membrane 1, molecules with a molecular diameter smaller than the pore diameter of the zeolite constituting the zeolite membrane and high polarity are preferentially adsorbed to the zeolite membrane and permeate through this membrane.

[0030] Among organometallic structure films, those that are particularly suitable are those that contain a CN crosslinked complex skeleton in their molecular structure, which has strong bonding forces between metal and organic molecules in its internal structure.

[0031] The gas separation container 2 is a container that houses the separation membrane 1 within its internal space. The shape of the gas separation container 2 is not limited as long as it has an internal space to house the separation membrane 1, but the gas separation container 2 may be formed in a cylindrical or rectangular shape, for example.

[0032] The internal space of the gas separation container 2 is divided into a first space 31 and a second space 32 by the separation membrane 1.

[0033] The gas separation container 2 may be made of a metal alloy such as an iron alloy, or a corrosion-resistant resin such as fluororesin.

[0034] The gas separation container 2 includes a raw material solution inlet 41 for introducing the raw material solution into the first space 31, an exhaust port 43 for exhausting unwanted gas from the first space 31 to the outside of the supply device 100 system, a carrier gas inlet 42 for introducing carrier gas into the second space 32, and an outlet 44 for discharging a mixed gas of carrier gas and product gas from the second space 32. The tip 73a of a drain pipe 73 for discharging the raw material solution from the first space 31 is inserted into the first space 31 of the gas separation container 2.

[0035] The first space 31 is a spatial region partitioned by the inner wall of the gas separation container 2 and the separation membrane 1, or a spatial region partitioned by the separation membrane 1, for storing the raw material solution (solution L2) introduced from the raw material solution inlet 41. The first space 31 is partitioned so that the raw material solution stored in the first space 31 and the separation membrane 1 are in contact. That is, the separation membrane 1 is positioned in contact with the raw material solution.

[0036] It is desirable that the first space 31 contains both a gas phase and a liquid phase (raw material solution). The gas phase may be nitrogen, air, or product gas.

[0037] The second space 32 is a separate spatial region from the first space 31 within the internal space of the gas separation container 2, which is partitioned by the inner wall of the gas separation container 2 and the separation membrane 1, or partitioned by the separation membrane 1, for receiving the raw material gas that has permeated through the separation membrane 1.

[0038] The second space 32 is adjacent to the first space 31 via the separation membrane 1. The raw material gas separated from the raw material solution stored in the first space 31 by the separation membrane 1 flows into the second space 32. The raw material gas that flows into the second space 32 mutually diffuses with the carrier gas introduced into the second space 32 via the carrier gas inlet 42 (described later) to form a mixed gas. The mixed gas is then sent to downstream equipment via the outlet 44 (described later) (the above is an example of the sending process).

[0039] In this embodiment, the gas separation container 2 is formed in a cylindrical shape, and its axis is positioned along the horizontal direction. The separation membrane 1 is a cylindrical body 10, which is housed in the internal space of the gas separation container 2. The cylindrical body 10 is positioned so that its axis is aligned along the horizontal direction.

[0040] In this embodiment, the second space 32 is the space inside the cylindrical body 10 (separation membrane 1), partitioned by the cylindrical body 10. The first space 31 is the internal space of the gas separation container 2, excluding the second space 32. The cylindrical body 10 is configured such that at least a portion of it is immersed in the raw material solution (solution L2) stored in the second space 32. Figure 1 illustrates the case where the entire cylindrical body 10 is immersed in the raw material solution. As a result, the separation membrane 1 is in contact with the raw material solution stored in the second space 32.

[0041] By bringing the raw material solution of the product gas into contact with the gas separation membrane 1, the product gas permeates through the separation membrane 1, thereby separating (evaporating) the product gas from the raw material solution (an example of a separation process). In this embodiment, the evaporation of the product gas through the separation membrane 1 is included in the concept of the product gas permeating through the separation membrane 1.

[0042] The raw material solution inlet 41 is an inlet for introducing the raw material solution (solution L1) from the raw material container 70 into the first space 31. The raw material solution inlet 41 connects the liquid supply pipe 72, which is a pipe that supplies the raw material solution from the raw material container 70 to the first space 31, to the first space 31, allowing the raw material solution to be introduced into the first space 31 from the raw material container 70 and the liquid supply pipe 72. The raw material container 70 may be successively replenished with raw material solution via the pipe 71 from, for example, a raw material solution preparation tank located upstream of the process.

[0043] The drain pipe 73 is a pipe that discharges the raw material solution (solution L2) as waste liquid (solution L3) from the first space 31 to the outside of the supply device 100 system. The drain pipe 73 is immersed in the raw material solution (solution L2) stored in the first space 31, and draws up the raw material solution from its base end 73a, discharging it as waste liquid to a waste liquid treatment device or the like outside the supply device 100 system.

[0044] In the gas separation container 2, the raw material gas components are separated from the raw material solution (solution L2) stored in the first space 31 by the separation membrane 1, thereby reducing the raw material gas components in the raw material solution. Therefore, new raw material solution is introduced into the first space 31, for example, continuously, through the raw material solution inlet 41. The raw material solution, from which the raw material gas components have been reduced, is then discharged as waste liquid (solution L3) outside the supply device 100 system via the drain pipe 73.

[0045] The exhaust port 43 is an outlet for discharging waste gas (gas G3) from the first space 31 to the outside of the supply device 100 system. In the first space 31, product gas may vaporize from the raw material solution, or solvent components may volatilize. The exhaust port 43 discharges these product gases and solvent gases as waste gas from the first space 31. The exhaust port 43 connects the first space 31 to an exhaust pipe 74 that sends the waste gas to an exhaust gas treatment device or the like outside the supply device 100 system. The exhaust port 43 is positioned so as not to come into contact with the raw material solution stored in the first space 31.

[0046] The carrier gas inlet 42 is an inlet for introducing carrier gas (gas G1), for example, supplied from the upstream side of the process, into the second space 32. The carrier gas inlet 42 connects the carrier gas supply pipe 82, which is a pipe supplying carrier gas from the upstream side, to the second space 32, allowing the carrier gas to be introduced into the second space 32 from the carrier gas supply pipe 82. The carrier gas introduced into the second space 32 from the carrier gas inlet 42 mutually diffuses with the product gas within the second space 32, becoming a mixed gas of carrier gas and product gas.

[0047] The outlet 44 is an outlet that sends the mixed gas (gas G2) from the second space 32 to equipment downstream of the process. The outlet 44 connects the mixed gas supply pipe 84, which is piping that supplies the mixed gas to equipment downstream of the process, to the second space 32.

[0048] Ports and piping such as the raw material solution inlet 41, carrier gas inlet 42, exhaust port 43, outlet port 44, liquid supply pipe 72, drain pipe 73, exhaust pipe 74, carrier gas supply pipe 82, and mixed gas supply pipe 84 may be made of metal alloys such as iron alloys or corrosion-resistant resins such as fluororesin.

[0049] In the second space section 32, the raw material gas separated from the raw material solution (solution L2) stored in the first space section 31 is mixed with the carrier gas introduced from the carrier gas inlet 42, and this mixed gas, at the concentration required by the downstream equipment, is sent from the outlet 44 to the downstream equipment.

[0050] The heating device 20 is a device equipped with a heating mechanism and heat source for heating the separation membrane 1 (an example of a heating process). The heating device 20 may heat the separation membrane 1 and the raw material solution (solution L2) stored in the first space 31 via the gas separation container 2. In other words, the heating device 20 may heat the gas separation container 2.

[0051] The heating device 20 may, for example, use an electric heater or a steam heater as a heating mechanism or heat source. The heating device 20 may also be a device that uses a heating mechanism that utilizes electromagnetic induction or radiant heat transfer.

[0052] The heating device 20 may be installed in the gas separation container 2, for example, so as to cover at least a portion of the outer surface of the gas separation container 2.

[0053] In the supply device 100 of this embodiment, the heating device 20 can heat the gas separation container 2, the separation membrane 1, and the raw material solution (solution L2). This makes it easier for the product gas in the raw material solution to permeate the separation membrane 1 more selectively.

[0054] Specifically, when the separation membrane 1 is heated, the components of the product gas are selectively adsorbed onto the separation membrane 1, making it easier for the product gas to selectively permeate through the separation membrane 1. The components of the product gas adsorbed onto the separation membrane 1 are further facilitated by the heating of the separation membrane 1, as surface diffusion of the product gas components within the separation membrane 1 is promoted, thereby accelerating permeation through the separation membrane 1. The components of the product gas that have permeated from the first space 31 to the second space 32 of the separation membrane 1 are further detached from the separation membrane 1 and diffused into the second space 32, especially when the separation membrane 1 is heated. The detachment and diffusion of the product gas components on the second space 32 side of the separation membrane 1 are promoted, making it even easier for the product gas to selectively permeate through the separation membrane 1. In this way, the heating process during the separation process improves the efficiency of separating the product gas from the raw material solution.

[0055] A concrete example of the effect of the heating process is as follows. For example, when a zeolite membrane is used as separation membrane 1, molecules with a molecular diameter smaller than the pore size of the zeolite and high polarity (molecules of the product gas components) are adsorbed onto separation membrane 1 (zeolite) preferentially over other molecules. At this time, heating separation membrane 1 can promote the adsorption, desorption, and surface diffusion of these molecules, allowing for the selective separation of the product gas. For example, if a mixed solution of hydrazine and an organic solvent is used as the raw material solution and brought into contact with a CHA-type zeolite membrane as separation membrane 1, hydrazine molecules smaller than the pore size of the zeolite (0.38 nm to 0.40 nm) are selectively adsorbed onto separation membrane 1 (preferentially over organic solvent molecules). Under heating conditions, when separation membrane 1 is heated, hydrazine repeatedly adsorbs and desorbs within separation membrane 1, causing hydrazine to permeate through separation membrane 1. In this way, hydrazine can be selectively separated (evaporated) from the mixed solution.

[0056] Furthermore, for example, if a mixed solution of formic acid and an organic solvent is used as the raw material solution and brought into contact with an MFI-type zeolite membrane as the separation membrane 1, formic acid molecules smaller than the pore size of the MFI-type zeolite will be selectively adsorbed onto the separation membrane 1. Similar to the case of hydrazine described above, under heating conditions in which the separation membrane 1 is heated, formic acid can be selectively separated (evaporated).

[0057] Furthermore, when a zeolite membrane is used as the separation membrane 1 of the supply device 100, the raw material gases that can be selectively separated (evaporated) are not limited to the hydrazine and formic acid exemplified above.

[0058] The heating device 20 heats the gas separation container 2 to, for example, 30°C to 200°C, preferably 30°C to 150°C. That is, the heating device 20 heats the separation membrane 1 to 30°C to 200°C, preferably 30°C to 150°C. By keeping the separation membrane 1 within the temperature range of 30°C to 200°C, the product gas is efficiently separated from the raw material solution. If the separation membrane 1 is within the temperature range of 30°C to 150°C, the product gas may be separated from the raw material solution even more efficiently.

[0059] The heating device 20 may be controlled to vary the amount of heating to maintain the gas separation container 2, separation membrane 1, or first space 31 at a constant temperature, or to reach a predetermined target temperature. In this case, temperature sensors for measuring the temperature of the gas separation container 2, separation membrane 1, or first space 31 may be attached to them, and the amount of heating by the heating device 20 may be controlled based on the measurement results of these temperature sensors. For example, a temperature sensor 29 for measuring the temperature of the separation membrane 1 may be installed on the separation membrane 1, and the amount of heating by the heating device 20 to heat the gas separation container 2 may be controlled based on the temperature of the separation membrane 1 measured by this temperature sensor 29.

[0060] The temperature of the separation membrane 1 may be determined by measuring the temperature of the raw material solution (solution L2) stored in the first space 31. For example, the temperature of the raw material solution stored in the first space 31 may be considered as the temperature of the separation membrane 1. Specifically, in order to measure the temperature of the separation membrane 1, a temperature sensor may be provided in the gas separation container 2, inserted within the space of the first space 31 and in contact with the raw material solution stored in the first space 31.

[0061] The amount of heating by this heating device 20 may be controlled, for example, based on the detection result of the concentration of the product gas contained in the mixed gas by the concentration sensor 89, which will be described later.

[0062] As an example of a case where, within a certain temperature range, an increase in the temperature of the separation membrane 1 makes it easier for the product gas to selectively permeate the separation membrane 1, and a decrease in the temperature of the separation membrane 1 makes it more difficult for the product gas to permeate the separation membrane 1, the heating device 20 may control the amount of heating as follows.

[0063] For example, if the concentration of product gas in the mixed gas is higher than the target value, the heating device 20 may reduce the amount of heating to lower the temperature of the gas separation container 2, the separation membrane 1, or the first space 31. Conversely, for example, if the concentration of product gas in the mixed gas is lower than the target value, the heating device 20 may increase the amount of heating to raise the temperature of the gas separation container 2, the separation membrane 1, or the first space 31. The amount of heating may be controlled so that the concentration of product gas in the mixed gas remains constant.

[0064] In other words, the amount of heating may be controlled based on the temperature of the gas separation container 2, the separation membrane 1, or the first space 31, and the concentration of the product gas contained in the mixed gas. For example, the temperature of the separation membrane 1 may be kept within the range of 30°C to 150°C, while the amount of heating may be controlled based on the detection result of the concentration of the product gas contained in the mixed gas.

[0065] The liquid level sensor 21 is a detection device that detects the liquid level height of the raw material solution (solution L2) stored in the first space 31. The liquid level sensor 21 can be of any type as long as it is capable of detecting the liquid level height of the raw material solution (solution L2). As an example, the liquid level sensor 21 can be an ultrasonic level sensor that detects the liquid level position using ultrasound, a laser level sensor that detects the liquid level position using a laser, or a float level sensor that detects the liquid level position using a float. The liquid level sensor 21 may be installed at an appropriate position in the gas separation container 2 depending on the liquid level detection method.

[0066] The liquid volume control mechanism 5 is a mechanism that controls the liquid level of the raw material solution (solution L2) stored in the first space 31 based on the detection result of the liquid level sensor 21. The liquid volume control mechanism 5 may include a supply and discharge mechanism for supplying the raw material solution to the first space 31 or for discharging the raw material solution from the first space 31.

[0067] The liquid volume control mechanism 5 controls the liquid level of the raw material solution, thereby controlling (adjusting) the liquid level of the raw material solution in contact with the separation membrane 1. Through this control by the liquid volume control mechanism 5, for example, the liquid level of the raw material solution in contact with the separation membrane 1 can be kept constant.

[0068] In some cases, the rate of permeation of the product gas through the separation membrane 1 can be adjusted by controlling the liquid level of the raw material solution in contact with the separation membrane 1. For example, by controlling the liquid level of the raw material solution in contact with the separation membrane 1, it may be possible to maintain a constant rate of permeation of the product gas through the separation membrane 1. Maintaining a constant rate of permeation of the product gas through the separation membrane 1 makes it easier to maintain a constant concentration of the product gas in the mixed gas.

[0069] In this embodiment, the liquid volume control mechanism 5 may include, as a supply and discharge mechanism, a liquid supply mechanism 51 installed in the raw material container 70, piping 71, drain pipe 73, and liquid supply pipe 72, which supplies raw material solution (solution L1) from the raw material container 70 to the first space 31, and a liquid supply mechanism 52 installed in the drain pipe 73, which discharges raw material solution (solution L2) from the first space 31 to the outside of the system as waste liquid (solution L3).

[0070] Examples of the liquid delivery mechanism 51 include a liquid delivery pump and a flow control valve.

[0071] An example of the liquid delivery mechanism 52 is a liquid delivery pump or a flow control valve.

[0072] The liquid volume control mechanism 5 controls the operation of the liquid supply mechanisms 51 and 52 (e.g., liquid supply volume, liquid supply output, valve opening) based on the liquid level sensor 21's detection of the liquid level of the raw material solution (solution L2), thereby controlling the liquid level of the raw material solution (e.g., maintaining a constant liquid level).

[0073] Furthermore, the liquid volume control mechanism 5 may control the residence time of the raw material solution (solution L2) stored in the first space 31. This residence time control may be performed by controlling the supply and discharge mechanism, similar to the control of the liquid level of the raw material solution performed by the liquid volume control mechanism 5 described above. By controlling the residence time, the concentration of the product gas component in the raw material solution stored in the first space 31 can be adjusted (for example, kept constant).

[0074] When the supply device 100 is supplying the mixed gas, the concentration of the product gas in the raw material solution (solution L2) stored in the first space 31 is lower than the concentration of the product gas in the raw material solution (solution L1) supplied from the raw material container 70. If the concentration of the product gas component in the raw material solution is low, the rate of permeation of the product gas through the separation membrane 1 will be slower. If the concentration of the product gas component in the raw material solution is high, the rate of permeation of the product gas through the separation membrane 1 will be faster. Therefore, the liquid volume control mechanism 5 can adjust the rate of permeation of the product gas through the separation membrane 1 by controlling the residence time of the raw material solution (solution L2) stored in the first space 31 and thereby adjusting the concentration of the product gas component in the raw material solution.

[0075] The concentration sensor 89 is a device for measuring the concentration of the product gas contained in the mixed gas (gas G2). The concentration sensor 89 may be appropriately selected depending on the type of product gas, and any type that can measure the concentration of the product gas contained in the mixed gas is acceptable. As an example, the concentration sensor 89 may be an optical gas concentration meter using ultraviolet light (e.g., vacuum ultraviolet light) or infrared light, or an ultrasonic gas concentration meter.

[0076] The concentration sensor 89 may be installed, for example, in a mixed gas supply pipe 84 to measure the concentration of the product gas contained in the mixed gas flowing through the mixed gas supply pipe 84.

[0077] The pressure control mechanism 6 controls the pressure of the mixed gas in the second space 32 based on the detection result of the concentration of the product gas contained in the mixed gas by the concentration sensor 89. The pressure control mechanism 6 may include a discharge rate control mechanism that controls the flow rate of the mixed gas (gas G2) discharged from the outlet 44.

[0078] The pressure control mechanism 6 controls the pressure of the mixed gas in the second space 32, thereby controlling (adjusting) the pressure difference between the pressure in the space on the first space 31 side (pressure of the raw material solution) and the pressure in the space on the second space 32 side (pressure of the mixed gas) in the separation membrane 1 (hereinafter referred to as the pressure difference in the separation membrane 1). Through the control by the pressure control mechanism 6, for example, the pressure difference in the separation membrane 1 can be kept constant.

[0079] In some cases, the rate of permeation of the product gas through the separation membrane 1 can be adjusted by controlling the pressure difference across the separation membrane 1. For example, by controlling the pressure difference across the separation membrane 1, it may be possible to maintain a constant rate of permeation of the product gas through the separation membrane 1. Maintaining a constant rate of permeation of the product gas through the separation membrane 1 makes it easier to maintain a constant concentration of the product gas in the mixed gas.

[0080] If the rate of permeation of the product gas through the separation membrane 1 decreases, and as a result the concentration of the product gas in the mixed gas falls below the target value, the pressure control mechanism 6 can adjust the pressure of the mixed gas in the second space 32 to increase the pressure difference in the separation membrane 1, which may increase the rate of permeation of the product gas through the separation membrane 1.

[0081] If the rate of permeation of the product gas through the separation membrane 1 becomes too high, causing the concentration of the product gas in the mixed gas to exceed the target value, the pressure control mechanism 6 can adjust the pressure of the mixed gas in the second space 32 to reduce the pressure difference in the separation membrane 1, which may slow down the rate of permeation of the product gas through the separation membrane 1.

[0082] The pressure control mechanism 6 controls the pressure of the mixed gas in the second space 32, thereby controlling the pressure difference in the separation membrane 1 and adjusting the rate of permeation of the product gas through the separation membrane 1. Furthermore, by controlling the pressure of the mixed gas in the second space 32, the pressure control mechanism 6 adjusts the rate of permeation of the product gas through the separation membrane 1, thereby controlling (for example, keeping constant) the concentration of the product gas contained in the mixed gas (gas G2).

[0083] In this embodiment, the pressure control mechanism 6 may include a mixed gas supply pipe 84 and a valve device 61, such as a flow control valve or a pressure control valve, installed in the mixed gas supply pipe 84 to control the flow rate of the mixed gas passing through it, as a discharge volume control mechanism.

[0084] The pressure control mechanism 6 can control the pressure of the mixed gas in the second space 32 by controlling the flow rate of the mixed gas flowing through the mixed gas supply pipe 84, that is, by controlling the flow rate of the mixed gas (gas G2) discharged from the outlet 44.

[0085] The pressure control mechanism 6 controls the operation of the valve device 61 (e.g., valve opening) based on the detection result of the concentration of the product gas contained in the mixed gas by the concentration sensor 89, thereby controlling the flow rate of the mixed gas (gas G2) discharged from the outlet 44 and controlling the pressure of the mixed gas in the second space 32.

[0086] The valve device 61 can be controlled, for example, by increasing its valve opening to increase the pressure of the mixed gas in the second space 32. The valve device 61 can also be controlled, for example, by decreasing its valve opening to decrease the pressure of the mixed gas in the second space 32.

[0087] As described above, an efficient gas supply device and gas supply method can be provided.

[0088] [Another embodiment] (1) In the above embodiment, the separation membrane 1 in the supply device 100 is described as a cylindrical body 10 formed in a cylindrical shape, housed in the internal space of the gas separation container 2, and the cylindrical body 10 is described as being immersed in the raw material solution. Furthermore, the second space 32 was described as the space inside the cylindrical body 10 (separation membrane 1) partitioned by the cylindrical body 10 (separation membrane 1). However, the separation membrane 1 is not limited to being formed in a cylindrical shape.

[0089] As shown in Figure 2, the separation membrane 1 may be flat. The second space 32 may be a separate spatial region from the first space 31 in the internal space of the gas separation container 2, which is partitioned by the inner wall of the gas separation container 2 and the separation membrane 1.

[0090] In the example shown in Figure 2, a flat separation membrane 1 divides the internal space of the gas separation container 2 into a first space 31 located above the separation membrane 1 and a second space 32 located below the separation membrane 1. The raw material solution stored in the first space 31 is in contact with the upper surface of the separation membrane 1.

[0091] (2) In the above embodiment, it was explained that the liquid volume control mechanism 5 controls the liquid level of the raw material solution stored in the first space 31 (for example, by keeping the liquid level constant). It was also explained that the liquid volume control mechanism 5 may control the residence time of the raw material solution (solution L2) stored in the first space 31.

[0092] The liquid volume control mechanism 5 may control the liquid level of the raw material solution stored in the first space 31 and the residence time of the raw material solution stored in the first space 31, as illustrated above, based on the detection results of the concentration of the product gas contained in the mixed gas by the concentration sensor 89.

[0093] For example, if the concentration of the product gas contained in the mixed gas falls below the target value, the liquid volume control mechanism 5 may control the system by raising the liquid level of the raw material solution stored in the first space 31 or by shortening the residence time of the raw material solution stored in the first space 31. If the concentration of the product gas contained in the mixed gas falls above the target value, the liquid volume control mechanism 5 may control the system by lowering the liquid level of the raw material solution stored in the first space 31 or by lengthening the residence time of the raw material solution stored in the first space 31.

[0094] Furthermore, the configurations disclosed in the above embodiments (including other embodiments, the same applies hereinafter) can be applied in combination with configurations disclosed in other embodiments, as long as no inconsistencies arise. In addition, the embodiments disclosed herein are illustrative, and the embodiments of the present invention are not limited thereto, and can be modified as appropriate without departing from the object of the present invention. [Industrial applicability]

[0095] The present invention can be applied to gas supply devices and gas supply methods. [Explanation of Symbols]

[0096] 1: Separation membrane 10: Cylindrical body 100: Feeding device 2: Gas separation vessel 20: Heating device 21: Liquid level sensor 29: Temperature sensor 31:First space part 32:Second space part 41: Raw material solution inlet 42: Carrier gas inlet 43: Exhaust vent 44: Outlet 5: Liquid volume control mechanism 51:Liquid mechanism 52:Liquid mechanism 6: Pressure control mechanism 61: Valve device 70: Raw material container 71: Piping 72:Liquid supply pipe 73: Drain pipe 73a:Tip 74: Exhaust pipe 82: Carrier gas supply pipe 84: Mixed gas supply pipe 89: Concentration sensor G1: Gas G2: Gas G3: Gas L1: Solution L2: Solution L3: Solution

Claims

1. A gas separation membrane that permeates the product gas, A gas separation container containing the separation membrane, The system includes a heating device for heating the separation membrane, The aforementioned gas separation container is A first space for storing the raw material solution of the product gas, The first space and the second space separated by the separation membrane, A carrier gas inlet that communicates with the second space and introduces carrier gas into the second space, A gas supply device having an outlet that communicates with the second space and discharges a mixed gas of the carrier gas and the product gas from the second space.

2. The gas supply device according to claim 1, wherein the separation membrane is positioned in contact with the raw material solution.

3. The gas supply device according to claim 1, wherein the raw material solution is a solution containing a raw material component consisting of polar molecules as a raw material for the product gas.

4. The raw material solution contains hydrazine, hydrogen peroxide, or formic acid as raw material components. The gas supply device according to claim 3, wherein the mixed gas comprises hydrazine, hydrogen peroxide, or formic acid as the product gas.

5. The gas supply apparatus according to any one of claims 1 to 4, wherein the separation membrane comprises at least one of a zeolite membrane and an organometallic structure membrane.

6. A liquid level sensor for detecting the liquid level height of the raw material solution in the first space, A gas supply device according to any one of claims 1 to 4, further comprising a liquid volume control mechanism that controls the liquid level height of the raw material solution based on the detection result of the liquid level sensor.

7. The gas supply device according to claim 6, wherein the liquid volume control mechanism includes a supply and discharge mechanism for supplying the raw material solution to the first space or discharging the raw material solution from the first space.

8. A concentration sensor for measuring the concentration of the product gas contained in the mixed gas, The gas supply device according to claim 6, further comprising a pressure control mechanism for controlling the pressure of the mixed gas in the second space based on the detection result of the concentration sensor.

9. The gas supply device according to claim 8, wherein the pressure control mechanism includes a discharge volume control mechanism that controls the flow rate of the mixed gas discharged from the outlet.

10. A separation step involves bringing the raw material solution of the product gas into contact with a gas separation membrane and separating the product gas from the raw material solution by allowing it to pass through the separation membrane. A heating step for heating the separation membrane, The process includes a discharge step in which a carrier gas is introduced into the product gas separated in the separation step, and a mixed gas of the product gas and the carrier gas is discharged. The heating step is a gas supply method performed during the separation step.

11. The gas supply method according to claim 10, wherein the raw material solution is a solution containing a raw material component consisting of polar molecules as a raw material for the product gas.

12. The raw material solution contains hydrazine, hydrogen peroxide, or formic acid as raw material components. The gas supply method according to claim 11, wherein the mixed gas comprises hydrazine, hydrogen peroxide, or formic acid as the product gas.

13. The gas supply method according to any one of claims 10 to 12, wherein at least one of a zeolite membrane and an organometallic structure membrane is used as the separation membrane.

14. The gas supply method according to any one of claims 10 to 12, wherein the separation step controls the liquid level of the raw material solution that comes into contact with the separation membrane.

15. The gas supply method according to claim 14, wherein in the delivery step, the pressure of the delivered mixed gas is controlled based on the concentration of the product gas contained in the mixed gas.

Images